Compositions containing carbon black and expanded graphite, as well as molded articles and substrate coatings containing same, their use and methods for reducing volume resistivity and providing electromagnetic interference shielding in addition to thermal conductivity - Patents.com

Abstract

The present invention is directed to compositions comprising carbon black and expanded graphite, and to coatings for molded articles and substrates comprising the compositions.The present invention also relates to their use and methods for reducing electrical resistivity and providing electromagnetic interference shielding in addition to thermal conductivity.The compositions of the present invention allow high electrical conductivity, EMI shielding performance and thermal conductivity without compromising rheological properties such as flowability or viscosity, measured for example as melt flow rate, or mechanical properties such as impact resistance, tensile strength or elongation at break.

Description

[Technical field]

[0001] The present invention is directed to compositions comprising carbon black and expanded graphite, and to molded articles and substrate coatings comprising the compositions. The present invention also relates to their use and methods for reducing electrical resistivity and providing electromagnetic interference shielding as well as thermal conductivity. [Background technology]

[0002] It is well known in the art to use fillers or additives to fine-tune the physical and chemical properties of polymer compositions and products containing or made from said polymer compositions. For example, carbon, silicon and metal based fillers have been used to reduce electrical resistivity and provide electromagnetic interference shielding as well as thermal conductivity. Electrical resistivity, ρ, also sometimes called electrical resistivity or specific electrical resistance, is a material property related to the degree of resistance of a material to electric current, expressed in SI units ohm·m or ohm·cm (Ω·m or Ω·cm, respectively). Volume resistivity is usually determined according to ASTM D-991, ASTM D-4496, ISO3915, or ISO1853 standard test methods. A material with low resistivity is one that readily conducts electric current. Thermal conductivity is expressed in SI units W m -1 *K -1 or W cm -1 *K -1 Thermal conductivity is a material property that quantifies a material's ability to conduct heat, expressed as a percentage. Materials with high thermal conductivity are very efficient at conducting heat. The thermal conductivity of a material is generally determined by standard tests according to ASTM E1461 or ISO22007.

[0003] Electromagnetic interference (EMI) is a physical phenomenon that occurs when an external source affects an electrical circuit through electromagnetic induction, capacitive coupling or conduction. EMI disrupts or even completely degrades the performance of the electrical circuit. EMI becomes a big problem when a large number of electronic components are used in, for example, medical, military, aerospace or automotive applications. The increasing use of electromagnetic waves, for example for electronic equipment on one side and wireless communication on the other side, increases the risk of unwanted crosstalk. To reduce or even completely eliminate the negative effects of EMI on electrical circuits, electromagnetic shielding, also called EMI shielding, is used. Electromagnetic shielding is usually achieved by electrically conductive or magnetic enclosures placed around electrical devices to isolate them from their environment. A common approach to EMI shielding is to use housings made from plastics with conductive additives or metal-based shielding materials (e.g., metal coatings). Composite materials are also known for EMI shielding applications.

[0004] The EMI shielding performance or EMI shielding effectiveness (EMI SE) of a material is generally expressed as the attenuation in decibels (dB) of electromagnetic waves at a certain frequency. EMI SE can be determined by standard tests such as ASTM D-4935 or IEE299 or methods derived therefrom. The EMI shielding performance of a material depends on several factors, including the electrical resistivity of the material, or its reciprocal, electrical conductivity. In the art, electrical conductivity and EMI shielding of composite materials is achieved by reducing the electrical resistivity of the composite material, for example, by adding conductive additives or fillers. Typical conductive additives or fillers known in the art are metal-based, silicon-based, or carbon-based, such as metal powders, metal flakes, or metal fibers, glass fibers, silicon fibers, natural graphite, artificial graphite, surface-modified graphite, graphite nanoplatelets, multi-walled carbon nanotubes, single-walled carbon nanotubes, carbon nanostructures, or metal-coated graphite. The properties of the conductive additive, such as shape, particle size, morphology, and aspect ratio, affect the conductivity of the material.

[0005] In this context, it is also known to use carbon black or expanded graphite as carbon-based conductive fillers. The structure of carbon black consists of primary particles made of concentrically arranged successive layers of hexagonally arranged carbon atoms containing small graphitic or turbostratic regions. The primary particles, which are approximately spherical in shape with an average diameter of several tens of nanometers, are fused together by successive carbon layers forming covalently bonded rigid aggregates. These aggregates exhibit a three-dimensional branched structure of primary particles arranged in chains, fibers or tufts, with sizes up to several hundreds of nanometers. A characteristic feature of conductive carbon black is the large size of the aggregate structure. Carbon black is widely used as an additive in polymers or compound compositions to provide electrical conductivity and EMI shielding. For example, Chinese Patent Application Publication No. 105885226 relates to a network cable insulation material containing carbon black to provide electromagnetic interference shielding.

[0006] Graphite is the most common allotrope of carbon and is characterized by good electrical, thermal and lubricating properties. Graphite powder is a suitable filler to improve the conductivity and friction properties of polymer composites. The term "graphitic carbon" includes various types of carbon powders with different levels of crystallinity, such as natural and artificial graphite. Natural graphite from mineral deposits occurs in three main forms: flake graphite, lump or scaly graphite, and amorphous graphite. Artificial graphite is produced from natural or petroleum carbon precursors in a high-temperature process that converts the amorphous carbon into carbon with a higher structural order.

[0007] Expanded graphite is an exfoliated form of graphite (Herold et al. 1994; Herold A, Petitjean D, Furdin G, Klatt M (1994) Exfoliation of graphite intercalation compounds: classification and discussion of the processes from new experimental data relative to graphite acid compounds. Mater Sci Forum 152-153:281-287 (Soft chemistry routes to new materials). The manufacturing process is based on the hot exfoliation of graphite intercalation compounds formed by treatment of graphite flakes with strong acids in the presence of an oxidizing agent. The most prominent graphite intercalation compounds used in industrial processes are graphite sulfate, Cm+HSO4n, which are prepared by reacting graphite flakes with concentrated sulfuric acid, hydrogen peroxide, ammonium peroxydisulfate, and nitric acid or chromic acid as oxidizing agents. H2SO4. Under these chemical conditions, the graphite is oxidized and, at the same time, sulfate anions and sulfate molecules are inserted between the graphite layers. Not all the graphite interlayers are necessarily occupied by guest species, but there are different stages of intercalation compounds. The stages that can be achieved depend on the chemical conditions, but usually the actual composition can vary, resulting in the non-stoichiometries typical of these graphite salts. Other reagents that can be used are nitric acid, chloric acid and nitric acid in acetic acid. The resulting graphite salt is isolated by filtration, washing and drying. Expansion of graphite salts occurs at temperatures above 300°C. On an industrial scale, the process is carried out by thermal shock, where the material is briefly exposed to temperatures above 700°C, causing decomposition of guest anions and acidic molecules between the graphite layers into gaseous products that exfoliate the graphite layers. Alternatively, microwave radiation can be used for the exfoliation process. After expansion, the powder consists of coarse, "worm-like" shaped grains. Usually, expanded graphite cannot be used in this form due to its extremely low bulk density, so it is ground to fine particle size or compressed into graphite foil or graphite "paper".The graphite particles resulting from the milling of expanded graphite are highly anisotropic (high aspect ratio) and extremely effective as conductive additives at low loadings. Particulate expanded graphite material in particular has shown advantages for incorporation into polymers using industrial feed mixing equipment (WO 2012 / 020099). The largest industrial application of exfoliated graphite is in seals and gaskets from graphite foils impregnated into polymers.

[0008] Expanded graphite is known to provide electrical conductivity, thermal conductivity, and to have a positive effect on lubrication performance. Advantageously, expanded graphite may be used at a lower loading compared to standard graphite, and still achieve the same benefits. Expanded graphite has also been known for use in polymer composites for many years (see, for example, U.S. Patent Nos. 1,137,373 and 1,191,383, and U.S. Patent Nos. 4,946,892 and 5,582,781).

[0009] US Patent No. 4,530,949 relates to a housing for electrical or electronic equipment prepared from an organic thermosetting resin molding composition containing expanded graphite in combination with glass fibers. The moldings provide resistivity of 0.5 ohm·cm or less and measured attenuation of 32-64 dB at frequencies between 50-1000 MHz. However, unfortunately, the compositions according to Examples 1-3 of US Patent No. 4,530,949 contain expanded graphite in combination with glass fibers and are not suitable for light-weight applications. It is also known in the art that thermosetting resins generally allow for lower percolation thresholds of conductive fillers such as carbon black and expanded graphite compared to thermoplastic resins. In other words, in thermosetting resins, electrical conductivity can be achieved at lower conductive filler loadings compared to thermoplastic resins. It is also known that thermosetting resins containing mixtures of carbon black and expanded graphite are generally difficult to process at high filler loadings. No. 4,704,231 describes a composite containing low density exfoliated graphite flakes in a polymer matrix that provides an electrical resistivity of the composite of less than 0.5 ohm·cm. Unfortunately, however, the low density exfoliated graphite flakes cannot be used at high loadings in thermoplastic resins because they result in poor processability. US 2006 / 0148965 is directed to expanded graphite for use, inter alia, in polymer composites. However, the composites of US 2006 / 0148965 disadvantageously provide resistivity greater than 10 ohm·cm, and not less. Also, composites containing up to 30% by weight of carbon black are reported to provide resistivities of 100 ohm·cm or greater. Thus, the composites of US 2006 / 0148965 are not capable of effective conductivity, and therefore effective EMI shielding.

[0010] Also, blends of carbon-based additives, such as carbon nanotubes and carbon black or graphene or graphene-like or graphite, in polymeric matrices are known to provide improved conductivity and sometimes better mechanical properties.However, the disadvantage of using conductive fillers such as carbon nanotubes and carbon black or graphene or graphene-like or graphite is that high loadings are usually required to provide good electrical and / or thermal conductivity.However, high loadings of conductive fillers such as carbon nanotubes and carbon black or graphene or graphene-like or graphite result in poor processability, for example due to high viscosity.

[0011] Furthermore, the use of carbon black in combination with expanded graphite in formulation compositions is known in the art. For example, Korean Patent Application Publication No. 2018 / 0022398 relates to a heat-dissipating polymer composite material containing a thermally conductive carbonaceous material, such as a heating pad having carbon nanotubes (CNTs), graphene nanoplates (GNPs), and expanded graphite (EG) uniformly dispersed in the polymer. The heating pad is also described as providing electromagnetic interference shielding, but not quantified. Furthermore, carbon nanotubes often have poor dispersibility in the polymer, resulting in a high percolation threshold. Also, carbon nanotubes are usually avoided because they are known to cause health hazards. Furthermore, the composite material according to Korean Patent Application Publication No. 2018 / 0022398 suffers from the reality that a combination of three conductive additives is required, which is neither resource- nor cost-efficient.

[0012] As another example, U.S. Patent No. 11,024,849 describes fast-chargeable lithium-ion and lithium-metal batteries that include polymer foams that contain electrically conductive carbonaceous materials, such as expanded graphite, carbon black, or combinations thereof, among others. However, U.S. Patent No. 11,024,849 does not provide any information regarding electromagnetic interference shielding or thermal conductivity. An article by Leao et al., Journal of Polymers and the Environment, 2020, 28, pp. 2021-2100, https: / / doi.org / 10.1007 / s10924-020-01753-4, addresses the electromagnetic interference shielding effectiveness of conductive polyvinylidene fluoride (rPVDF) composites containing carbon black, expanded graphite, and their mixtures. In particular, Leao et al. report that a composite containing 5% by weight of a combination of carbon black and expanded graphite in a ratio of 1.5 (3% by weight carbon black: 2% by weight expanded graphite) provides approximately 97% electromagnetic wave attenuation, corresponding to approximately -15 dB at a frequency of 12.3 GHz. The rPVDF composite is also described as providing acceptable processability. Unfortunately, however, the composite by Leao et al. does not provide attenuation greater than -15 dB, requiring improvement in electromagnetic interference shielding.

[0013] Object of the Invention Improvement of the electrical and EMI shielding properties as well as the thermal conductivity of a composite material can in principle be achieved by increasing the content of conductive additives (conductive fillers). However, this approach is limited, since high filler loadings have a negative effect on the rheological and mechanical properties of the composite material, such as viscosity, tensile strength or elongation at break. At too high a filler loading, the processability of the composition is therefore reduced. For example, at high filler loadings, for example above 50% by weight relative to the total weight of the composition, extrusion becomes difficult and injection molding is often even impossible. Also, a too high filler loading is disadvantageous, since it increases the weight of the composition or the article obtained by producing it. The present invention aims to overcome the drawbacks of the prior art described above. Against this background, the present invention aims to optimize the electrical conductivity, EMI shielding efficiency and thermal conductivity on the one hand, and the amount of conductive additive used, i.e. the conductive filler loading, on the other hand. In particular, it is desirable to reduce the conductive filler loading in the composite, and to maintain or even improve the electrical conductivity, EMI shielding efficiency and thermal conductivity of the composite. Furthermore, it is desirable to have compositions available that allow high electrical conductivity, EMI shielding performance and thermal conductivity without compromising the rheological properties, such as flowability or viscosity, measured for example as melt flow rate, or the mechanical properties, such as impact resistance, tensile strength or elongation at break. It is also desirable to have compositions available that allow lightweight materials with high electrical conductivity, EMI shielding performance and thermal conductivity. Summary of the Invention

[0014] To achieve one or more or all of these objectives, the present invention provides a composition comprising carbon black and expanded graphite according to claim 1 or claim 6 or claim 11. Furthermore, the present invention also provides a shaped article according to claim 17 or a coated substrate according to claim 18, comprising a composition as claimed in the claims. Furthermore, the present invention is directed to the use of the compositions or shaped articles or substrate coatings according to the present claims to provide EMI shielding, volume resistivity and / or thermal conductivity (see claims 19 to 24). Advantageous embodiments of the compositions, shaped articles, coated substrates, uses and methods of the invention are the subject of the respective dependent claims. [Brief description of the drawings]

[0015] [Figure 1] FIG. 1 shows the results of melt flow rate measurements at 230° C. and 5 kg for polypropylene composites with different combinations and ratios of carbon black and expanded graphite fillers. [Figure 2A]FIG. 1 shows the results of melt flow rate measurements at 240° C. and 5 kg for polyamide composites with different loadings of carbon black (Ensaco® 250G) and expanded graphite (Timrex® C-THERM™ 011) and synthetic graphite (Timrex® KS44). [Figure 2B] FIG. 1 shows the results of melt flow rate measurements at 240° C. and 12.5 kg for polyamide composites with different loadings of carbon black (Ensaco® 250G) and expandable graphite (Timrex® C-THERM™ 011) and combinations thereof. [Diagram 3] FIG. 1 shows a plot of volume resistivity (ohms·cm) measured for polypropylene samples prepared from compositions containing conductive fillers including a blend of carbon black (Ensaco® 250G) and expanded graphite (Timrex® C-THERM™ 011) or synthetic graphite (Timrex® SFG44) at a total filler amount of 30 wt.% based on the total weight of the composition versus the fraction of expanded graphite or synthetic graphite in the conductive additive filler blend. [Figure 4] FIG. 1 shows a plot of the volume resistivity (ohm·cm) measured for polyamide samples containing different conductive fillers versus the total additive content in wt % relative to the total weight of the composition. [Figure 5A]FIG. 1 shows the corrected EMI shielding efficiency depending on polypropylene composites having the following compositions in the order of decreasing shielding efficiency: (i) sample PP-5.3 with 15% by weight carbon black (Ensaco® 250G) / 15% by weight expandable graphite (Timrex® C-THERM™ 011); (ii) sample PP-5.10 with 10% by weight carbon black (Ensaco® 250G) / 10% by weight expandable graphite (Timrex® C-THERM™ 011) / 10% by weight carbon fiber (Tenax A HT P802 3mm); (iii) sample PP-5.10 with 15% by weight carbon black (Ensaco® 250G) / 15% by weight carbon fiber (Tenax A HT P802 3mm); (iv) sample PP-5.6 containing 15% by weight carbon black (Ensaco® 250G) / 15% by weight expandable graphite (Timrex® C-THERM™ 301); (v) sample PP-5.7 containing 15% by weight carbon black (Ensaco® 250G) / 15% by weight expandable graphite (Timrex® C-THERM™ MAX HD); (vi) sample PP-5.8 containing 7.5% by weight carbon black (Ensaco® 350G) / 15% by weight expandable graphite (Timrex® C-THERM™ 011); and (vii) neat polypropylene without any conductive additive. [Figure 5B] FIG. 1 shows the corrected versus uncorrected EMI shielding efficiency for selected polypropylene compositions, in order of decreasing EMI shielding efficiency, including: (i) sample PP-5.3 with 15 wt% carbon black (Ensaco® 250G) / 15 wt% expandable graphite (Timrex® C-THERM™ 011); (ii) sample PP-5.1 with 30 wt% carbon black (Ensaco® 250G); (iii) sample PP-5.5 with 30 wt% expandable graphite (Timrex® C-THERM™ 011); and (iv) a control sample comprising neat polypropylene with no conductive additive. [Figure 6A]FIG. 1 shows the thermal conductivity of polypropylene composites containing blends of varying amounts of carbon black (Ensaco® 250G) and expandable graphite (Timrex® C-THERM™ 011). [Figure 6B] FIG. 1 shows the thermal conductivity of polyamide composites containing different amounts of various fillers. [Figure 7A] FIG. 1 shows the tensile modulus for polypropylene composites containing varying amounts of blends of carbon black (Ensaco® 250G) and expandable graphite (Timrex® C-THERM™ 011) or carbon black (Ensaco® 250G) and synthetic graphite (Timrex® SFG44). [Figure 7B] FIG. 1 shows the tensile modulus for polyamide composites containing different amounts of various fillers. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0016] (definition) In the context of the present invention, the term "electrical resistivity", also sometimes referred to as electrical resistivity ρ, volume resistivity or specific electrical resistance, is a material property related to the degree of resistance of a material to an electric current, expressed in SI units ohm·m or ohm·cm (Ω·m or Ω·cm, respectively). Volume resistivity is usually determined according to the ASTM D-4496 standard test method. A material with low resistivity is one that readily conducts electric current. In the context of the present invention, the term "thermal conductivity" is expressed in SI units W m -1 *K -1 or W cm -1 *K -1 Thermal conductivity refers to a material property that quantifies a material's ability to conduct heat, expressed as a percentage. Materials with high thermal conductivity are very efficient at conducting heat. The thermal conductivity of a material is generally determined by standard tests according to ASTM E1461 or ISO22007. Thermal conductivity can be measured in in-plane and thickness modes.

[0017] In the context of the present invention, the term "electromagnetic interference (EMI)" is a physical phenomenon that occurs when an external source affects an electrical circuit by electromagnetic induction, electrostatic coupling or conduction. EMI disrupts or even completely degrades the performance of the electrical circuit. Similarly, in the context of the present invention, the term "electromagnetic interference shielding" refers to the ability of a material to reduce or even completely eliminate the negative effects of EMI on an electrical circuit. In this regard, in the context of the present invention, the term "EMI shielding effectiveness (EMI SE)" refers to the EMI shielding performance of a material, generally expressed as the attenuation in decibels (dB) of electromagnetic waves at a certain frequency. EMI SE is determined in a specific frequency range by standard testing, for example according to ASTM D-4935 or a method derived therefrom. In the context of the present invention, EMI SE is measured according to ASTM D-4935 at frequencies between 10 and 1000 MHz, or a method derived therefrom as detailed in the paper E. Hariya and U. Massahiro, "Instruments for Measuring Shielding Effectiveness", EMC 1984 Tokyo. In the context of the present invention, the terms "conductive additive" and "conductive filler" are used interchangeably and refer to materials that are added to a polymer, such as a formulation, polymer binder or resin, to provide thermal and / or electrical conductivity to the polymer. Conductive additives or conductive fillers are known to those skilled in the art and may be carbonaceous, metal-based or hybrid materials in various forms, such as powders, fibers or flakes.

[0018] (Embodiments of the invention) In a first aspect, the present invention provides a composition comprising carbon black and expanded graphite. The composition of the present invention is characterized by one or more of the following: The composition of the present invention comprises carbon black in an amount of 3 to 40, preferably 5 to 35, more preferably 10 to 30, even more preferably 12 to 26, and most preferably 13 to 18% by weight relative to the total weight of the composition. The composition of the present invention comprises expandable graphite in an amount of 3 to 50, preferably 3 to 40, more preferably 3 to 35, even more preferably 3 to 30, still more preferably 3.5 to 20, particularly more preferably 4 to 18, particularly still more preferably 5 to 17, and most preferably 7 to 15 mass %, relative to the total mass of the composition. The composition comprises carbon black and expandable graphite in a combined amount of 10 to 50, preferably 17 to 45, more preferably 19 to 40, even more preferably 20 to 35, still more preferably 22 to 34, particularly preferably 24 to 31, and most preferably 25 to 30 mass %, based on the total mass of the composition. The mass % ratio of carbon black to expandable graphite relative to the total mass of the composition of the present invention is in the range of 0.1 to 9, preferably 0.33 to 9, more preferably 0.4 to 9, even more preferably 0.4 to 7, still more preferably 0.4 to 5, particularly more preferably 0.4 to 3, particularly still more preferably 0.4 to 2, and most preferably 0.6 to 1.7.

[0019] The composition of the present invention is 950m 2 ·g -1 Less than 850m, preferably 2 ·g -1 Less than 700m, preferably 2 ·g -1 Less than 600m, even more preferably 2 ·g -1 Less than 500m, most preferably 2 ·g -1 less than 40-800, preferably 50-800, more preferably 30-100, even more preferably 50-80, most preferably 60-70 m 2 ·g -1 and optionally a primary particle size, measured according to ASTM D3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or -1 Less than 390ml g -1 Less than 380ml g -1Less than 370ml g -1 Less than 350ml g -1 less than 100-330, preferably 150-230, more preferably 170-210, even more preferably 180-200, and most preferably 185-195 ml g -1 The carbon blacks are characterized by one or more oil absorption numbers, OAN, as measured in accordance with ASTM D-2414, in the range of 0.1 to 1.0.

[0020] The composition of the present invention has a particle size distribution D as measured according to ISO 13220 of 5 to 1000, preferably 20 to 800, more preferably 30 to 700, even more preferably 50 to 600, still more preferably 70 to 500, particularly preferably 80 to 250, and most preferably 85 to 150 μm. 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, particularly preferably 0.16 to 0.45, and most preferably 0.16 to 0.25 g cm -3 and bulk density, as measured in accordance with ASTM D-7481.

[0021] In a preferred embodiment, the composition of the present invention comprises: (a) carbon black in an amount of 3 to 40, preferably 5 to 35, more preferably 10 to 30, even more preferably 12 to 26, and most preferably 13 to 18 mass %, based on the total mass of the composition; and (b) expandable graphite in an amount of 3 to 50, preferably 3 to 40, more preferably 3 to 35, even more preferably 3 to 30, still more preferably 3.5 to 20, particularly more preferably 4 to 18, especially still more preferably 5 to 17, and most preferably 7 to 15 mass %, based on the total mass of the composition.

[0022] In another preferred embodiment, the composition of the present invention comprises: (a) carbon black; and (b) expandable graphite, wherein the carbon black is 950 mm 2 ·g -1Less than 850m, preferably 2 ·g -1 Less than 700m, preferably 2 ·g -1 Less than 600m, even more preferably 2 ·g -1 Less than 500m, most preferably 2 ·g -1 less than 40-800, preferably 50-800, more preferably 30-100, even more preferably 50-80, most preferably 60-70 m 2 ·g -1 and optionally a primary particle size measured according to ASTM D3849-14a of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or -1 Less than 390ml g -1 Less than 380ml g -1 Less than 370ml g -1 Less than 350ml g -1 less than 100-330, preferably 150-230, more preferably 170-210, even more preferably 180-200, and most preferably 185-195 ml g -1 and / or the expanded graphite is characterized by one or more of a particle size distribution D as measured according to ISO 13220 of 5 to 1000, preferably 20 to 800, more preferably 30 to 700, even more preferably 50 to 600, still more preferably 70 to 500, particularly preferably 80 to 250, and most preferably 85 to 150 μm. 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, particularly preferably 0.16 to 0.45, and most preferably 0.16 to 0.25 g cm -3or bulk density as measured in accordance with ASTM D-7481.

[0023] In yet another preferred embodiment, the composition of the present invention comprises carbon black and expandable graphite, wherein the weight percent ratio of carbon black to graphite relative to the total weight of the composition is in the range of 0.1 to 9, preferably 0.33 to 9, more preferably 0.4 to 9, even more preferably 0.4 to 7, even more preferably 0.4 to 5, particularly more preferably 0.4 to 3, especially still more preferably 0.4 to 2, and most preferably 0.6 to 1.7; and the carbon black is 2 ·g -1 Less than 850m, preferably 2 ·g -1 Less than 700m, preferably 2 ·g -1 Less than 600m, even more preferably 2 ·g -1 Less than 500m, most preferably 2 ·g -1 less than 40-800, preferably 50-800, more preferably 30-100, even more preferably 50-80, most preferably 60-70 m 2 ·g -1 and optionally a primary particle size, measured according to ASTM D-3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or a primary particle size, measured according to ASTM D-3849-14a, of 400 ml g -1 Less than 390ml g -1 Less than 380ml g -1 Less than 370ml g -1 Less than 350ml g -1 less than 100-330, preferably 150-230, more preferably 170-210, even more preferably 180-200, and most preferably 185-195 ml g -1and / or the expanded graphite is characterized by one or more of a particle size distribution D as measured according to ISO 13220 of 5 to 1000, preferably 20 to 800, more preferably 30 to 700, even more preferably 50 to 600, still more preferably 70 to 500, particularly preferably 80 to 250, and most preferably 85 to 150 μm. 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, particularly preferably 0.16 to 0.45, and most preferably 0.16 to 0.25 g cm -3 or bulk density as measured in accordance with ASTM D-7481.

[0024] In another preferred embodiment, it is also provided that the composition according to the invention comprises one or more fillers selected from the group consisting of carbon-based fillers selected from the group consisting of metal powders, metal flakes, glass fibers, silicon fibers, carbon conductive additives, natural graphite, artificial graphite, surface modified graphite, graphite nanoplatelets, multi-walled carbon nanotubes, single-walled carbon nanotubes, carbon nanostructures, metal coated graphite, and combinations thereof. Such fillers may be used to optimize and fine-tune the chemical and physical properties of the composition.

[0025] In another preferred embodiment, it is also provided that the composition comprises a polymer, preferably a polyolefin, preferably a polymer selected from the group consisting of polyolefins selected from polyethylene, polypropylene and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethylmethacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymer, polyester, polycarbonate, polyketone, polysulfone, unsaturated polyester, polyurethane, polycyclopentadiene, silicone, rubber, thermoset resin, thermoplastic resin, coating binder and combinations thereof.In this way, the composition of the present invention can be applied to a wide range of polymers.

[0026] In a second aspect, the present invention provides a molded article of a composite material comprising a composition according to the invention as described above. In a third aspect, the present invention provides a substrate coated with a coating comprising the composition of the present invention. The shaped articles or coatings for substrates of the present invention may comprise a polymer selected from the group consisting of polyolefins, preferably selected from polyethylene, polypropylene and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethylmethacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymers, polyesters, polycarbonates, polyketones, polysulfones, unsaturated polyesters, polyurethanes, polycyclopentadiene, silicones, rubbers, thermosets, thermoplastics, coating binders and combinations thereof. In a preferred embodiment of the inventive coating for molded articles or substrates, the carbon black and expanded graphite are dispersed in the polymer, which provides an equal distribution of the conductive additive in the polymer and provides certain favorable effects such as EMI shielding efficiency or thermal conductivity.

[0027] In a fourth aspect, the present invention provides a ferroelectric material having an electromagnetic interference (EMI) shielding of at least 20 dB, preferably at least 30 dB, more preferably at least 40 dB, measured according to ASTM D-4935 at frequencies between 10 and 1000 MHz, or a method derived therefrom as detailed in the paper E. Hariya and U. Massahiro, “Instruments for Measuring Shielding Effectiveness”, EMC 1984 Tokyo; a volume resistivity, measured according to ASTM D-4496, of less than 1000 ohm·cm, preferably less than 100 ohm·cm, more preferably less than 10 ohm·cm, and most preferably less than 1 ohm·cm; and / or a volume resistivity, measured according to ASTM D-4496, of less than 1000 ohm·cm, preferably less than 100 ohm·cm, more preferably less than 10 ohm·cm, and most preferably less than 1 ohm·cm; -1 K -1 More than 0.7 W m -1 K -1 More than 0.9 W m -1 K -1 More preferably, 1.1 W m -1 K -1 More than 1.3 W m -1 K -1 More preferably still, 1.5 W m -1 K -1 More particularly, and even more preferably, 1.7 W m -1 K -1 More preferably still, 2.0 W m -1 K -1 More preferably still, 2.5 W m -1 K -1 More than 3.0 W m -1 K -1 More than 4.0 W m -1 K -1 More preferably still, 5.0 W m -1 K -1 More preferably, 6.0 W m -1 K -1 More than 7.0 W m -1 K -1The present invention provides a use of a composition, a shaped article or a coated substrate according to the present invention as described above to provide one or more in-plane thermal conductivities, measured according to ASTM E1461, of greater than 0.01%.

[0028] In a fifth aspect, the present invention provides a method for providing an electromagnetic interference (EMI) shielding in a polymeric composition using a composition, molded article or coated substrate according to the invention as described above, the EMI shielding being at least 20 dB, preferably at least 30 dB, more preferably at least 40 dB, measured according to standard test method ASTM D-4935 at frequencies between 10 MHz and 1000 MHz, or a method derived therefrom as detailed in the paper E. Hariya and U. Massahiro, “Instruments for Measuring Shielding Effectiveness”, EMC 1984 Tokyo.

[0029] In a sixth aspect, the present invention provides a method for providing a volume resistivity, as measured according to standard test method ASTM D-4496, in a polymeric composition using a composition, a shaped article, or a coated substrate according to the present invention as described above, of less than 1000 ohm·cm, preferably less than 100 ohm·cm, more preferably less than 10 ohm·cm, and most preferably less than 1 ohm·cm. In a seventh aspect, the present invention provides a polymeric composition using a composition, molded article or coated substrate according to the invention as described above, the composition comprising: -1 K -1 More than 0.7 W m -1 K -1 More than 0.9 W m -1 K -1 More preferably, 1.1 W m -1 K -1 More than 1.3 W m -1 K -1 More preferably still, 1.5 W m -1 K -1More particularly, and even more preferably, 1.7 W m -1 K -1 More preferably still, 2.0 W m -1 K -1 More preferably still, 2.5 W m -1 K -1 More than 3.0 W m -1 K -1 More than 4.0 W m -1 K -1 More preferably still, 5.0 W m -1 K -1 More preferably, 6.0 W m -1 K -1 More than 7.0 W m -1 K -1 The present invention provides a method for providing an in-plane thermal conductivity, as measured in accordance with ASTM E1461, that is greater than or equal to 1.

[0030] In a further preferred embodiment, the use or method of providing electromagnetic interference (EMI) shielding of the present invention improves the EMI shielding by at least 10 dB, preferably at least 20 dB, more preferably at least 25 dB, even more preferably at least 30 dB, still more preferably at least 35 dB, particularly more preferably at least 40 dB, most preferably at least 45 dB, in particular from 10 to 80 dB, preferably from 15 to 70 dB, more preferably from 18 to 60 dB, in particular more preferably from 20 to 55 dB, even more preferably from 25 to 50 dB, in particular even more preferably from 27 to 50 dB, still more preferably from 30 to 50 dB, in particular even more preferably from 31 to 45 dB, most preferably from 35 to 42 dB, when compared to a reference material not comprising carbon black, expanded graphite or other conductive fillers or additives, in particular the composition according to the present invention as described above.

[0031] In a further preferred embodiment, the use or method providing the volume resistivity of the present invention reduces the volume resistivity by a factor of 1.3 to 109, preferably 1.5 to 108, more preferably 2 to 107, particularly preferably 2 to 106, even more preferably 2 to 105, particularly still more preferably 3 to 105, even more preferably 3 to 104, particularly still more preferably 5 to 104, even more preferably 7 to 104, even more preferably 7 to 103, particularly still more preferably 10 to 103, particularly still more preferably 15 to 103, even more preferably 50 to 103 and most preferably 102 to 103, when compared to a reference material not containing carbon black, expanded graphite or other conductive fillers or additives, in particular the composition according to the present invention as described above.

[0032] In a further preferred embodiment, the in-plane thermal conductivity providing use or method of the present invention increases the in-plane thermal conductivity by a factor of 2, preferably 3, more preferably 4, particularly preferably 5, even more preferably 6, particularly even more preferably 7, even more preferably 8, particularly even more preferably 9, even more preferably 10, even more preferably 12, particularly even more preferably 14, particularly even more preferably 16, even more preferably 18, even more preferably 20, particularly even more preferably 25, particularly even more preferably 30, even more preferably 40 and most preferably 50, when compared to a reference material not containing carbon black, expanded graphite or other conductive fillers or additives, in particular the compositions according to the present invention described above.

[0033] In summary, the subject matter of the present invention described above advantageously makes it possible to optimize both the amount of conductive additive and the desired properties of the composition, such as electrical conductivity, EMI shielding efficiency and in-plane thermal conductivity, without compromising the rheological and mechanical properties. It is intended that all material contained in the above description be construed as illustrative and not in a limiting sense. Thus, certain changes may be made in the compositions, uses and methods described above without departing from the scope of the invention. The invention will be further illustrated by the following examples which illustrate the preparation of the compositions and their corresponding properties without limiting the invention. EXAMPLES

[0034] (Materials used) polymer: - Polypropylene commercially available as "PP412 MN40"; - A polyamide commercially available as "Technyl C246".

[0035] Additives: Conductive carbon black, commercially available from Imerys as "Ensaco® 250G", having an oil absorption number (OAN) of 190 mL / 100 g and an average molecular weight of 65 nm. 2 Characterized by BET specific surface area under nitrogen in g / g; Extra-Conductive Carbon Black, commercially available from Imerys as "Ensaco® 350G", 320 mL / 100 g OAN and 770 ml 2 Characterized by BET specific surface area under nitrogen in g / g; - Expanded graphite (high aspect ratio graphite), commercially available from Imerys as "Timrex® C-THERM™ 011"; D 90 Characterized by a particle size distribution of =90 μm; - Expanded graphite (high aspect ratio graphite), commercially available from Imerys as "Timrex® C-THERM™ 301"; D 90 Characterized by a particle size distribution of =30 μm; - Expanded graphite (high aspect ratio graphite), commercially available from Imerys as "Timrex® C-THERM™ MAX HD"; D 90 is characterized by a particle size distribution greater than 400 μm; - Synthetic graphite (low aspect ratio primary synthetic graphite), commercially available from Imerys as "Timrex® SFG44", approximately 5 m 2 BET specific surface area / g and D 90 Characterized by a particle size distribution of =50 μm; - low aspect ratio primary synthetic graphite, commercially available from Imerys as "Timrex® KS44", approximately 9 m 2 BET specific surface area under nitrogen and D 90 = 46 μm. - Carbon fiber, commercially available from Teijin Limited as "Tenax A HT P802 3mm", characterized by a fiber diameter of 7 μm and a pellet length of 8 mm.

[0036] Methods and equipment used: The melt flow rate (MFR) is measured at 5 kg and 230° C. by a melt flow tester, CEAST, according to standard ISO 1133. Other conditions used for the MFR measurement are given below.

[0037] The volume resistivity is measured using a Loresta GX instrument manufactured by Nitto Seiko Analytech Co., Ltd. using a 4-point ASP probe according to standard ASTM D4496. The EMI shield is made of a small compressed plate (150 x 150 mm) with a thickness of 2.3 to 2.4 mm. 2 The samples were tested at frequencies ranging from 10 MHz to 1 GHz according to the "TEM-t cell" method derived from ASTM D-4935 (details can be found in the paper E. Hariya and U. Massahiro, "Instruments for Measuring Shielding Effectiveness", EMC 1984 Tokyo). For all samples with attenuation above 25 dB, a correction factor was applied that corresponds to the theoretical value of an empty TEM-t cell as derived from the equivalent circuit. The thermal conductivity is measured using a Laserflash LFA447 from Netzsch according to standard ASTM E1461 at a temperature of 23° C. The measurements are performed both in-plane and through the film thickness with respect to the material flow during the platelet filling stage.

[0038] Tensile properties are measured using an Instron Dynamometer 5966 according to ISO 527. Formulations tested: A) Composition containing polypropylene (PP) A-1) PP composition containing a blend of CB and EG Carbon black (OAN = 190 mL / g and 65 m 2 Ensaco® 250G manufactured by Imerys, having a BET specific surface area under nitrogen of 1.0 mm / g, and expanded graphite (D 90 The polypropylene compositions listed in Table 1.1 were prepared with a final loading of conductive additive of 30 wt. % based on the total weight of the composition including different blends of Timrex® C-THERM™ 011 from Imerys having a .mu.m diameter of 1000 μm.

[0039] [Table 1]

[0040] A-2) PP composition containing further blends of conductive fillers For comparative testing, different types of carbon black (OAN = 190 mL / g and 65 m 2 Ensaco® 250G from Imerys with a BET specific surface area under nitrogen of 100 mL / 100 g or OAN = 320 mL / 100 g and 770 m 2 Ensaco® 350G from Imerys, which has a BET specific surface area under nitrogen of 1.0 mm / g, and different types of expanded graphite (D 90 = 90 μm Timrex® C-THERM™ 011 or D from Imerys 90 = Timrex® C-THERM™ 301 from Imerys with a D of 30 μm or greater than 400 μm90 Formulations were prepared with a final loading of conductive additive of 30% by weight based on the total weight of the composition (with the exception of sample PP-12 with 22.5% by weight based on the total weight of the composition) including different blends of Timrex® C-THERM™ MAX HD from Imerys with 100% by weight of PTFE; see samples PP-10 to PP-12), optionally with carbon fiber (Tenax A HT P802 3 mm from Teijin Ltd. with fiber diameter of 7 μm and pellet length of 8 mm) as further conductive additive (samples PP-13 to PP-14). See Table 1.2.

[0041] [Table 2]

[0042] A-3) PP composition containing a blend of CB and artificial graphite For comparative testing, carbon black (OAN = 190 mL / g and 65 m 2 Ensaco® 250G (Imerys) with a BET specific surface area under nitrogen of about 5 g / m 2 BET specific surface area and D 90 Formulations were prepared with a final loading of conductive additive of 30 wt. % based on the total weight of the composition, including different blends of “Timrex® SFG44 Primary Synthetic Graphite” from Imerys, characterized by a particle size distribution of 0.1 μm to 50 μm. See Table 1.3.

[0043] [Table 3]

[0044] B) Composition containing polyamide (PA) Using different final loadings of conductive additive and with different single component additives, or carbon black (OAN = 190 mL / g and 65 m 2 Ensaco® 250G (Imerys) with a BET specific surface area under nitrogen of 1 / g and expanded graphite (D90 Polyamide compositions listed in Table 2 were prepared using blends with Timrex® C-THERM™ 011 from Imerys having a diameter of about 9 mm. 2 BET specific surface area under nitrogen and D 90 A formulation was prepared containing Imerys' "Timrex® KS44" having a fiber diameter of 46 μm.

[0045] [Table 4]

[0046] Example 1: Preparation of the Complex Samples PP-1 to PP-17 and PA-1 to PA-13 described above are used as composites in at least some of the following examples, in which the composites are prepared by melt extrusion using a twin-screw extruder, Leistritz ZSE 27 mm, with an L / D ratio of 48, equipped with two side feeders. The polymer melt temperature is set at 240° C., the screw speed is fixed at 200 rpm, and the total output is 15 kg / h. Polypropylene, Sabic, PP412 MN40, is added to the main feeder. Conductive additives are added to the polymer melt using one or two side feeders fed by gravity feeders. The composites are extruded through a die, cooled by a water batch and granulated using a rotating cutting blade.

[0047] (Example 2: Preparation of test specimens (small plates)) Samples for volume resistivity, mechanical testing and thermal conductivity are prepared by injection molding using a Billion Proxima 50T. A LabTech press LPS20 is used to compress samples for EMI shielding testing. 150 x 150 x 2.4 mm 2 Small plates of are prepared.

[0048] (Example 3: Measurement of Viscosity (MFI)) The present inventors have found that blends of carbon black and expanded graphite, according to the present invention, advantageously provide acceptable rheological properties.

[0049] (3.1. Viscosity (MFI) data of polypropylene composition) [Table 5]

[0050] From the data presented in Table 3.1 and Figure 1, it can be derived that with increasing amount of carbon black in the conductive additive, the viscosity increases (the more carbon black in the conductive additive, the lower the MFI) and vice versa, with increasing amount of expanded graphite, the viscosity decreases (the more expanded graphite in the conductive additive, the higher the MFI).

[0051] Also, from samples PP-3.3, PP-3.6 and PP-3.7 with a CB:EG ratio of 1 containing different types of expandable graphite, D 90 It can be derived that Imerys' expanded graphite Timrex® C-THERM™ 011 having a .DELTA.=90 μm provides the lowest MFI (maximum viscosity) in blends with Ensaco® 250G carbon black. Additionally, the conductive additive blends containing carbon fiber provide a lower viscosity (higher MFI) than blends without carbon fiber.

[0052] (3.2. Viscosity (MFI) data of polyamide compositions) [Table 6]

[0053] The present inventors have found that polyamide compositions containing more than 10% by weight of carbon black (Ensaco® 250G) are very viscous and therefore more difficult to handle compared to polyamide compositions containing lower carbon black loadings or fillers other than carbon black such as expanded graphite or artificial graphite. Against this background, higher sample loads of 10 and 12.5 kg, respectively, were required for the measurement of the viscosity (determined as MFI) of samples PA-3.12 to PA-3.15 and sample PA-3.18.

[0054] The inventors of the present invention also found that sample PA-3.15 containing 30% by weight of carbon black (Ensaco® 250G) could not be injection molded, and a polyamide composition containing 15% by weight of carbon black (Ensaco® 250G) and 15% by weight of expandable graphite (Timrex® C-THERM™ 011) could no longer be extruded. According to the data presented in Table 3.2 above, at corresponding filler loadings, samples containing 10% by weight or more of expanded graphite exhibit lower viscosities (higher MFI) compared to samples containing exclusively carbon black at the same loadings.

[0055] (Example 4: Measurement of volume resistivity) The present inventors have found that blends of carbon black and expanded graphite according to the present invention advantageously provide superior conductivity.

[0056] (4.1. Volume resistivity data of polypropylene compositions) The volume resistivity of polypropylene compositions containing a blend of carbon black and expanded graphite as conductive additives at an additive loading of 30% by weight based on the total weight of the composition was measured (samples PP-4.1 to PP-4.9). For comparative testing, the volume resistivity of polypropylene compositions containing a blend of carbon black and artificial graphite as conductive additives at an additive loading of 30% by weight based on the total weight of the composition was measured (samples PP-4.10 to PP-4.12). See Table 4.1.

[0057] [Table 7] TIFF2024541271000009.tif101156

[0058] From table 4.1 and figure 3, it can be derived that samples PP-4.5 (CB:EG=1), PP-4.3 (CB:EG=3), PP-4.2 (CB:EG=6.9) and PP-4.4 (CB:EG=1.65) give the lowest volume resistivity of 9.23*E-1 ohm·cm, 6.68*E-1 ohm·cm, 6.0*E-1 ohm·cm and 6.67*E-1 ohm·cm respectively. Also, as can be derived from table 4.1 above, at equal additive loading of 30 wt% and carbon black to graphite ratio of 1, samples containing blend of carbon black and expanded graphite give significantly lower volume resistivity as compared to samples containing blend of carbon black and synthetic graphite. For example, samples PP-4.5, PP-4.10 and PP-4.11, which contain expanded graphite with a carbon black to graphite ratio of 1, gave volume resistivities of 9.23*E-1 ohm·cm, 1.37*E0 ohm·cm and 2.13*E0 ohm·cm respectively, which are significantly lower compared to the volume resistivity of 2.8*E0 ohm·cm measured for sample PP-4.15, which contains artificial graphite.

[0059] In particular, from Table 4.1 and Figure 3, it can be derived that the conductive additive containing a blend of carbon black and expanded graphite gives a lower volume resistivity compared to the single conductive additive fillers, i.e., exclusive carbon black or exclusive expanded graphite. This result suggests a synergistic effect of carbon black and expanded graphite on volume resistivity. (4.2. Volume resistivity data of polyamide compositions)

[0060] [Table 8]

[0061] As can be derived from Table 4.2 and Figure 4, for polyamide samples containing a single conductive additive, the volume resistivity decreases with increasing additive amount. This effect is more pronounced for samples containing carbon black and / or expanded graphite compared to samples containing artificial graphite. Most importantly, the present inventors have surprisingly found that blends of carbon black and expanded graphite, especially those containing a carbon black to expanded graphite ratio of 1, at a total filler loading of 25 wt%, partial amounts of 12.5 wt% carbon black (Ensaco® 250G) and 12.5 wt% expanded graphite (Timrex® C-THERM™ 011), respectively, provide a volume resistivity that is four orders of magnitude lower compared to the corresponding polyamide composition containing a single conductive additive. This result suggests a synergistic effect of carbon black and expanded graphite on the volume resistivity.

[0062] Example 5: Measurement of EMI shielding efficiency of polypropylene compositions The present inventors have discovered that blends of carbon black and expanded graphite according to the present invention advantageously provide superior EMI shielding. EMI shielding data was obtained for the polypropylene compositions at frequencies between 10 MHz and 1000 MHz. Selected data points for the corrected EMI shielding efficiency (attenuation) in dB are reproduced below in Table 5. Figure 5A is the corrected plot and Figure 5B is a plot of the corrected and uncorrected EMI shielding efficiency (attenuation) versus frequency taking into account more data points not shown in Table 5.

[0063] [Table 9] TIFF2024541271000012.tif227160 TIFF2024541271000013.tif227160 TIFF2024541271000014.tif145160

[0064] As can be derived from Table 5 and Figures 5A and 5B, the corrected EMI shielding efficiency of the tested polypropylene composites decreases in the following order: (i) sample PP-5.3 with 15% by weight carbon black (Ensaco® 250G) / 15% by weight expandable graphite (Timrex® C-THERM™ 011); (ii) sample PP-5.10 with 10% by weight carbon black (Ensaco® 250G) / 10% by weight expandable graphite (Timrex® C-THERM™ 011) / 10% by weight carbon fiber (Tenax A HT P802 3mm); (iii) sample PP-5.10 with 15% by weight carbon black (Ensaco® 250G) / 15% by weight carbon fiber (Tenax A HT P802 3mm); (iv) sample PP-5.6 containing 15 wt% carbon black (Ensaco® 250G) / 15 wt% expandable graphite (Timrex® C-THERM™ 301); (v) sample PP-5.7 containing 15 wt% carbon black (Ensaco® 250G) / 15 wt% expandable graphite (Timrex® C-THERM™ MAX HD); (vi) sample PP-5.8 containing 7.5 wt% carbon black (Ensaco® 350G) / 15 wt% expandable graphite (Timrex® C-THERM™ 011); (vii) a control sample containing neat polypropylene without any conductive additive.

[0065] Also, sample PP-5.3 containing 15% by weight carbon black (Ensaco® 250G) / 15% by weight expanded graphite (Timrex® C-THERM™ 011) exhibits an attenuation of about 40-45 dB in the frequency range of about 20 to about 1000 MHz. The inventors surprisingly found that this composition is even better than the composition containing carbon fiber, highlighting the exceptional EMI shielding performance of the composition according to the invention.

[0066] (Example 6: Measurement of thermal conductivity) The present inventors have found that blends of carbon black and expanded graphite according to the present invention advantageously provide good thermal conductivity as follows:

[0067] (6.1. Thermal Conductivity Data of Polypropylene Compositions) [Table 10]

[0068] As can be derived from Table 6.1 and Figure 6A, for polypropylene compositions containing a blend of carbon black and expanded graphite, both the film thickness as well as the in-plane conductivity increase with increasing amounts of expanded graphite (samples PP-6.1 to PP-6.5).

[0069] At equal additive loadings of 30 wt. % and a carbon black to expandable graphite ratio of 1 (i.e., samples PP-6.3, PP-6.6, and PP-6.7), D as the expandable graphite component was 90 Sample PP-6.3, which contains Timrex® C-THERM™ 011 from Imerys having a pore size of 0.05 μm, gives the highest thermal conductivity. Also, the use of carbon fibers results in poorer thermal conductivity compared to samples according to the invention that do not contain carbon fibers.

[0070] (6.2. Thermal Conductivity Data of Polyamide Compositions) [Table 11]

[0071] As can be derived from Table 6.2 and Figure 6B, both the in-plane and thickness thermal conductivities of polyamide samples containing expanded graphite are higher than those of polyamide samples containing synthetic graphite or carbon black at equal filler loadings. Additionally, sample PA-6.13, which contains a blend of 12.5 wt.% carbon black (Ensaco® 250G) and 12.5 wt.% expandable graphite (Timrex® C-THERM™ 011), provides similar in-plane thermal conductivity to sample PA-6.12, which contains 30 wt.% synthetic graphite.

[0072] Example 7: Measurement of mechanical properties: tensile strength The present inventors have found that blends of carbon black and expandable graphite according to the present invention advantageously provide good tensile strength.

[0073] (7.1. Tensile Strength Data of Polypropylene Composition) [Table 12]

[0074] The present inventors have surprisingly found that compositions according to the invention of carbon black and expanded graphite provide superior tensile properties when compared to blends of carbon black and synthetic graphite. As can be derived from Table 7.1 and Figure 7A, increasing the amount of expanded graphite in a polypropylene composition provides a higher elastic modulus (Young's modulus). Although to a lesser extent, this effect is also observed for compositions containing synthetic graphite. Also, at an equal filler amount of 30% by weight and an equal ratio of carbon black to expanded graphite and synthetic graphite, respectively, blends of carbon black and expanded graphite advantageously provide a higher elastic modulus (Young's modulus). (7.2. Tensile Strength Data of Polyamide Compositions)

[0075] [Table 13]

[0076] (References) International Publication No. 2012 / 020099 U.S. Patent No. 1,137,373 · U.S. Patent No. 1,191,383 U.S. Patent No. 4,946,982 · U.S. Patent No. 5,582,781 U.S. Patent No. 4,530,949 U.S. Patent No. 4,704,231 · U.S. Patent Application Publication No. 2006 / 0148965 ·US Patent Application Publication No. 2018 / 0022398 U.S. Patent No. 11,024,849 ·Leao et al. Journal of Polymers and the Environment, 2020, 28, pp. 2021-2100, https: / / doi.org / 10.1007 / s10924-020-01753-4

[0077] List of embodiments The first embodiment of the present invention is (a) carbon black in an amount of 3 to 40, or 5 to 35, or 10 to 30, or 12 to 26, or 13 to 18 weight percent based on the total weight of the composition; and (b) the composition comprises expanded graphite in an amount of 3 to 50, or 3 to 40, or 3 to 35, or 3 to 30, or 3.5 to 20, or 4 to 18, or 5 to 17, or 7 to 15 mass%, based on the total mass of the composition. A second embodiment of the invention relates to a composition according to the first embodiment, wherein the combined amount of carbon black and expandable graphite is from 10 to 50, or from 17 to 45, or from 19 to 40, or from 20 to 35, or from 22 to 34, or from 24 to 31, or from 25 to 30 wt.%, based on the total weight of the composition. A third embodiment of the present invention relates to a composition according to any of the first or second embodiments, wherein the weight percent ratio of carbon black to expandable graphite relative to the total weight of the composition is in the range of 0.1 to 9, or 0.33 to 9, or 0.4 to 9, or 0.4 to 7, or 0.4 to 5, or 0.4 to 3, or 0.4 to 2, or 0.6 to 1.7.

[0078] The fourth embodiment of the present invention relates to the composition according to any one of the first to third embodiments, wherein the carbon black is - 950m 2 ·g -1 Less than or equal to 850m 2 ·g -1 Less than or equal to 700m 2 ·g -1 Less than or equal to 600m 2 ·g -1 Less than or 500m 2 ·g -1 Less than 40-800, or 50-800, or 30-100, or 50-80, or 60-70 m 2 ·g -1 BET specific surface area under nitrogen measured according to ASTM D-3037 in the range of and, optionally, - a primary particle size, measured according to ASTM D-3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or - 400ml·g -1 Less than or equal to 390ml·g -1 Less than or equal to 380ml·g -1 , or 370 ml·g -1 Less than or equal to 350ml·g -1 Less than, in particular, 100-330, 150-230, 170-210, 180-200, or 185-195 ml·g -1 The oil absorption number (OAN), as measured in accordance with ASTM D-2414-01, is in the range of 0.1 to 1.0.

[0079] A fifth embodiment of the present invention relates to the composition according to any one of the first to fourth embodiments, wherein the expanded graphite is - particle size distribution D, measured according to ISO 13220, from 5 to 1000, or from 20 to 800, or from 30 to 700, or from 50 to 600, or from 70 to 500, or from 80 to 250, or from 85 to 150 μm 90 ; and / or - 0.01 to 1.00, or 0.02 to 0.9, or 0.05 to 0.7, or 0.1 to 0.55, or 0.13 to 0.50, or 0.16 to 0.45, or 0.16 to 0.25 g cm -3 or bulk density as measured in accordance with ASTM D-7481.

[0080] A sixth embodiment of the present invention comprises: (a) carbon black; and (b) containing expandable graphite; Carbon black is - 950m 2 ·g -1 Less than or equal to 850m 2 ·g -1 Less than or equal to 700m 2 ·g -1 Less than or equal to 600m 2 ·g -1 Less than or 500m 2 ·g -1 Less than 40-800, or 50-800, or 30-100, or 50-80, or 60-70 m 2 ·g -1 BET specific surface area under nitrogen, measured according to ASTM D-3037, in the range of; and, optionally, the following: - a primary particle size measured in accordance with ASTM D-3849-14a of 10 to 60, or 15 to 55, or 20 to 40, or 25 to 35 nm; and / or - 400ml·g -1 Less than or equal to 390ml·g -1 Less than or equal to 380ml·g -1 Less than or equal to 370ml·g -1 Less than or equal to 350ml·g -1 Less than, in particular, 100-330, 150-230, 170-210, 180-200, or 185-195 ml·g -1 an oil absorption number, OAN, as measured in accordance with ASTM D-2414, in the range of and / or Expandable graphite is: - particle size distribution D, measured according to ISO 13220, from 5 to 1000, or from 20 to 800, or from 30 to 700, or from 50 to 600, or from 70 to 500, or from 80 to 250, or from 85 to 150 μm 90 ; and / or - 0.01~1.00, or 0.02~0.9, or 0.05~0.7, or 0.1~0.55, or 0.13~0.50, or 0.16~0.45, or 0.16~0.25g cm -3 and bulk density as measured in accordance with ASTM D-7481.

[0081] A seventh embodiment of the present invention relates to the composition according to the sixth embodiment, comprising carbon black in an amount of 3 to 40, or 5 to 35, or 10 to 30, or 12 to 26, or 13 to 18% by weight relative to the total weight of the composition. An eighth embodiment of the present invention relates to a composition according to any of the sixth or seventh embodiments, comprising the expanded graphite in an amount of 3-50, or 3-40, or 3-35, or 3-30, or 3.5-20, or 4-18, or 5-17, or 7-15% by weight, relative to the total weight of the composition.

[0082] A ninth embodiment of the present invention relates to the composition according to any one of the sixth to eighth embodiments, comprising carbon black and expandable graphite in a combined amount of 10-50, or 17-45, or 19-40, or 20-35, or 22-34, or 24-31, or 25-30 wt.%, based on the total weight of the composition. A tenth embodiment of the present invention relates to the composition according to any one of the sixth to ninth embodiments, wherein the weight percent ratio of carbon black to graphite relative to the total weight of the composition is in the range of 0.1 to 9, or 0.33 to 9, or 0.4 to 9, or 0.4 to 7, or 0.4 to 5, or 0.4 to 3, or 0.4 to 2, or 0.6 to 1.7.

[0083] An eleventh embodiment of the present invention relates to a composition comprising carbon black and expanded graphite, wherein the weight percent ratio of carbon black to graphite relative to the total weight of the composition is in the range of 0.1 to 9, or 0.33 to 9, or 0.4 to 9, or 0.4 to 7, or 0.4 to 5, or 0.4 to 3, or 0.4 to 2, or 0.6 to 1.7; Carbon black is 950m 2 ·g -1 Less than or equal to 850m 2 ·g -1 Less than or equal to 700m 2 ·g -1 Less than or equal to 600m 2 ·g -1 Less than or 500m 2 ·g -1 Less than 40-800, or 50-800, or 30-100, or 50-80, or 60-70 m 2 ·g -1 BET specific surface area under nitrogen measured according to ASTM D-3037 in the range of; and, optionally, - primary particle size measured according to ASTM D-3849-14a of 10-60, or 15-55, or 20-40, or 25-35 nm; and / or - 400ml·g -1 Less than or equal to 390ml·g -1 Less than or equal to 380ml·g -1 Less than or equal to 370ml·g -1 Less than or equal to 350ml·g -1 Less than, in particular, 100-330, 150-230, 170-210, 180-200, or 185-195 ml·g -1 and characterized by one or more oil absorption numbers, as measured in accordance with ASTM D-2414, in the range of and / or Expandable graphite is - particle size distribution D, measured according to ISO 13220, from 5 to 1000, or from 20 to 800, or from 30 to 700, or from 50 to 600, or from 70 to 500, or from 80 to 250, or from 85 to 150 μm 90 ; and / or - 0.01~1.00, or 0.02~0.9, or 0.05~0.7, or 0.1~0.55, or 0.13~0.50, or 0.16~0.45, or 0.16~0.25g cm -3 or bulk density as measured in accordance with ASTM D-3037.

[0084] A twelfth embodiment of the present invention relates to the composition according to the eleventh embodiment, comprising carbon black in an amount of 3 to 40, or 5 to 35, or 10 to 30, or 12 to 26, or 13 to 18% by weight relative to the total weight of the composition. A thirteenth embodiment of the present invention relates to a composition according to any of the eleventh or twelfth embodiments, comprising the expanded graphite in an amount of 3-50, or 3-40, or 3-35, or 3-30, or 3.5-20, or 4-18, or 5-17, or 7-15% by weight, based on the total weight of the composition. A fourteenth embodiment of the present invention relates to the composition according to any one of the eleventh to thirteenth embodiments, comprising a combined amount of carbon black and expandable graphite of from 10 to 50, or from 17 to 45, or from 19 to 40, or from 20 to 35, or from 22 to 34, or from 25 to 30 wt.%, based on the total weight of the composition. A fifteenth embodiment of the present invention relates to the composition of any one of the first to fourteenth embodiments, comprising one or more further fillers selected from the group consisting of carbon-based fillers selected from the group consisting of metal powders, metal flakes, glass fibers, silicon fibers, carbon conductive additives, natural graphite, artificial graphite, surface modified graphite, graphite nanoplatelets, multi-walled carbon nanotubes, single-walled carbon nanotubes, carbon nanostructures, metal coated graphite, and combinations thereof.

[0085] A sixteenth embodiment of the present invention relates to the composition according to any one of the first to fifteenth embodiments, comprising a polymer, preferably a polyolefin, preferably a polymer selected from the group consisting of a polyolefin selected from polyethylene, propylene and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethyl methacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymer, polyester, polycarbonate, polyketone, polysulfone, unsaturated polyester, polyurethane, polycyclopentadiene, silicone, rubber, thermoset, thermoplastic, coating binder and combinations thereof. A seventeenth embodiment of the present invention relates to a molded article of a composite material comprising the composition according to any one of the first to sixteenth embodiments. An eighteenth embodiment of the present invention relates to a substrate coated with a coating comprising a composition according to any one of the first to sixteenth embodiments.

[0086] A 19th embodiment of the present invention relates to a shaped article according to the 17th embodiment or a coated substrate according to the 18th embodiment, comprising a polymer selected from the group consisting of polyolefins, preferably selected from polyethylene, polypropylene and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethylmethacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymer, polyester, polycarbonate, polyketone, polysulfone, unsaturated polyester, polyurethane, polycyclopentadiene, silicone, rubber, thermoset, thermoplastic, coating binder and combinations thereof. A twentieth embodiment of the present invention relates to a shaped article or a coated substrate according to the nineteenth embodiment, wherein the carbon black and the expandable graphite are dispersed in the polymer.

[0087] A 21st embodiment of the present invention comprises: - Electromagnetic interference (EMI) shielding of at least 20 dB, or at least 30 dB, or at least 40 dB, measured according to ASTM D-4935, or a method derived therefrom, as detailed in the paper E. Hariya and U. Massahiro, “Instruments for Measuring Shielding Effectiveness”, EMC 1984 Tokyo, at frequencies between 10 and 1000 MHz; - a volume resistivity, measured in accordance with ASTM D-4496, that is less than 1000 ohm·cm, or less than 100 ohm·cm, or less than 10 ohm·cm, or less than 1 ohm·cm; and / or - 0.5Wm -1 K -1 Exceeding 0.7Wm -1 K -1 Exceeding 0.9Wm -1 K -1 Exceeding 1.1 Wm -1 K -1 or more than 1.3 Wm -1 K -1 or more than 1.5Wm -1 K -1 or more than 1.7 Wm -1 K -1 or more than 2.0Wm -1 K -1 or more than 2.5Wm -1 K -1 Exceeding 3.0Wm -1 K -1 Exceeding 4.0Wm -1 K -1 Exceeding 5.0Wm -1 K -1 Exceeding 6.0Wm -1 K -1 Exceeding 7.0Wm -1 K -1The use of the composition according to any one of the first to sixteenth embodiments, or the shaped article according to any one of the seventeenth or nineteenth to twentieth embodiments, or the coated substrate according to any one of the eighteenth to twentieth embodiments, to provide one or more of an in-plane thermal conductivity, measured according to ASTM E1461, of greater than

[0088] A 22nd embodiment of the present invention relates to a method of providing an electromagnetic interference (EMI) shielding in a polymeric composition using a composition according to any one of the 1st to 16th embodiments, or in a shaped article according to any one of the 17th, 19th or 20th embodiments, or in a coated substrate according to any one of the 18th to 20th embodiments, of at least 20 dB, or at least 30 dB, or at least 40 dB, measured according to ASTM D-4935, or a method derived therefrom as detailed in the paper E. Hariya and U. Massahiro, “Instruments for Measuring Shielding Effectiveness”, EMC 1984 Tokyo, at frequencies between 10 MHz and 1000 MHz. A 23rd embodiment of the present invention relates to a method for providing a volume resistivity, measured according to standard test method ASTM D-4496, of less than 1000 ohm-cm, or less than 100 ohm-cm, or less than 10 ohm-cm, or less than 1 ohm-cm, in a polymeric composition using a composition according to any one of the 1 to 16 embodiments, or in a shaped article according to any one of the 17, 19 or 20 embodiments, or in a coated substrate according to any one of the 18 to 20 embodiments.

[0089] A 24th embodiment of the present invention relates to a polymeric composition using a composition according to any one of the first to sixteenth embodiments, or a shaped article according to any one of the seventeenth, nineteenth or twentieth embodiments, or a coated substrate according to any one of the eighteenth to twentieth embodiments, which has a thermal conductivity of 0.5 Wm2, measured according to ASTM E1461. -1 K -1Exceeding 0.7Wm -1 K -1 Exceeding 0.9Wm -1 K -1 Exceeding 1.1 Wm -1 K -1 or more than 1.3 Wm -1 K -1 or more than 1.5Wm -1 K -1 or more than 1.7 Wm -1 K -1 or more than 2.0Wm -1 K -1 or more than 2.5Wm -1 K -1 Exceeding 3.0Wm -1 K -1 Exceeding 4.0Wm -1 K -1 Exceeding 5.0Wm -1 K -1 Exceeding 6.0Wm -1 K -1 Exceeding 7.0Wm -1 K -1 The present invention relates to a method for providing an in-plane thermal conductivity of greater than

[0090] A 25th embodiment of the present invention relates to a use or method of providing electromagnetic interference (EMI) shielding according to any of the 21st or 22nd embodiments, which is improved by at least 10 dB, or at least 20 dB, or at least 25 dB, or at least 30 dB, or at least 35 dB, or at least 40 dB, or at least 45 dB, in particular by 10 to 80 dB, or 15 to 70 dB, or 18 to 60 dB, or 20 to 55 dB, or 25 to 50 dB, or 27 to 50 dB, or 30 to 50 dB, or 31 to 45 dB, or 35 to 42 dB, when compared to a reference material not comprising carbon black, expanded graphite or other conductive fillers or additives, in particular a composition according to any one of the 1 to 16 embodiments.

[0091] A 26th embodiment of the present invention relates to a use or method providing a volume resistivity according to any of the 21st or 23rd embodiment that is reduced by a factor of 1.3 to 10, or 1.5 to 10, or 2 to 10, or 2 to 10, or 2 to 10, or 3 to 10, or 3 to 10, or 5 to 10, or 7 to 10, or 7 to 10, or 10 to 10, or 15 to 10, or 50 to 10, or 10 to 10. A 27th embodiment of the present invention relates to a use or method providing an in-plane thermal conductivity according to any one of the 21st or 24th embodiments that is increased by a factor of 2, or 3, or 4, or 5, or 6, or 7, or 8, or 9, or 10, or 12, or 14, or 16, or 18, or 20, or 25, or 30, or 40, or 50, when compared to a reference material, in particular a composition according to any one of the 1st to 16th embodiments, that does not contain carbon black, expanded graphite or other conductive fillers or additives.

Claims

1. (a) carbon black in an amount of 3 to 40, preferably 5 to 35, more preferably 10 to 30, even more preferably 12 to 26, and most preferably 13 to 18, weight percent, based on the total weight of the composition; and (b) A composition comprising expanded graphite in an amount of 3 to 50, preferably 3 to 40, more preferably 3 to 35, even more preferably 3 to 30, still more preferably 3.5 to 20, particularly more preferably 4 to 18, especially even more preferably 5 to 17, and most preferably 7 to 15% by weight, based on the total weight of the composition.

2. 2. The composition of claim 1, wherein the combined amount of carbon black and expandable graphite is from 10 to 50, preferably from 17 to 45, more preferably from 19 to 40, even more preferably from 20 to 35, still more preferably from 22 to 34, especially more preferably from 24 to 31, and most preferably from 25 to 30 wt.%, based on the total weight of the composition.

3. 3. The composition according to claim 1 or 2, wherein the weight % ratio of carbon black to expandable graphite relative to the total weight of the composition is in the range of 0.1 to 9, preferably 0.33 to 9, more preferably 0.4 to 9, even more preferably 0.4 to 7, still more preferably 0.4 to 5, especially more preferably 0.4 to 3, especially even more preferably 0.4 to 2, and most preferably 0.6 to 1.

7.

4. Carbon black is - 950m 2 ・g -1 Less than 850m, preferably 2 ・g -1 Less than 700m, more preferably 2 ・g -1 less than, and even more preferably, 600 m 2 ・g -1 Less than 500m, most preferably 2 ・g -1 less than, in particular 40 to 800, preferably 50 to 800, more preferably 30 to 100, even more preferably 50 to 80, most preferably 60 to 70 m 2 ・g -1 BET specific surface area under nitrogen measured according to ASTM D-3037 in the range of and, optionally, a primary particle size, measured according to ASTM D-3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or - 400ml / g -1 Less than 390 ml g -1 less than, more preferably 380 ml g -1 less than, and even more preferably less than 370 ml g -1 less than, most preferably 350 ml g -1 less than, in particular 100 to 330, preferably 150 to 230, more preferably 170 to 210, even more preferably 180 to 200, most preferably 185 to 195 ml g -1 10. The composition of claim 1, characterized by one or more oil absorption numbers OAN, as measured in accordance with ASTM D-2414, in the range of:

5. Expanded graphite is a particle size distribution D, as measured according to ISO 13220, of from 5 to 1000, preferably from 20 to 800, more preferably from 30 to 700, even more preferably from 50 to 600, still more preferably from 70 to 500, particularly more preferably from 80 to 250, most preferably from 85 to 150 μm 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, especially more preferably 0.16 to 0.45, most preferably 0.16 to 0.25 g cm -3 10. The composition of claim 1, characterized by one or more of a bulk density, as measured in accordance with ASTM D-7481, of 0.01 to 0.01% by weight of the composition.

6. (a) carbon black; and (b) containing expanded graphite; Carbon black is - 950m 2 ・g -1 Less than 850m, preferably 2 ・g -1 Less than 700m, more preferably 2 ・g -1 less than, and even more preferably, 600 m 2 ・g -1 Less than 500m, most preferably 2 ・g -1 less than, in particular 40 to 800, preferably 50 to 800, more preferably 30 to 100, even more preferably 50 to 80, most preferably 60 to 70 m 2 ・g -1 BET specific surface area under nitrogen measured according to ASTM D-3037 in the range of and, optionally, the following: a primary particle size, measured according to ASTM D-3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or - 400ml / g -1 Less than 390 ml g -1 less than, more preferably 380 ml g -1 less than, and even more preferably less than 370 ml g -1 less than, most preferably 350 ml g -1 less than, in particular 100 to 330, preferably 150 to 230, more preferably 170 to 210, even more preferably 180 to 200, most preferably 185 to 195 ml g -1 an oil absorption number (OAN), as measured in accordance with ASTM D-2414, in the range of and / or Expanded graphite is: a particle size distribution D, as measured according to ISO 13220, of from 5 to 1000, preferably from 20 to 800, more preferably from 30 to 700, even more preferably from 50 to 600, still more preferably from 70 to 500, particularly more preferably from 80 to 250, most preferably from 85 to 150 μm 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, especially more preferably 0.16 to 0.45, most preferably 0.16 to 0.25 g cm -3 and a bulk density as measured in accordance with ASTM D-7481 standard.

7. 7. The composition of claim 6, comprising carbon black in an amount of 3 to 40, preferably 5 to 35, more preferably 10 to 30, even more preferably 12 to 26, and most preferably 13 to 18% by weight, relative to the total weight of the composition.

8. 7. The composition according to claim 6, comprising expanded graphite in an amount of 3 to 50, preferably 3 to 40, more preferably 3 to 35, even more preferably 3 to 30, still more preferably 3.5 to 20, particularly more preferably 4 to 18, especially still more preferably 5 to 17, and most preferably 7 to 15% by weight, relative to the total weight of the composition.

9. 7. The composition of claim 6, comprising carbon black and expandable graphite in a combined amount of 10 to 50, preferably 17 to 45, more preferably 19 to 40, even more preferably 20 to 35, still more preferably 22 to 34, especially more preferably 24 to 31, and most preferably 25 to 30 wt. %, based on the total weight of the composition.

10. 7. The composition of claim 6, wherein the weight % ratio of carbon black to graphite relative to the total weight of the composition is in the range of 0.1 to 9, preferably 0.33 to 9, more preferably 0.4 to 9, even more preferably 0.4 to 7, still more preferably 0.4 to 5, especially more preferably 0.4 to 3, especially even more preferably 0.4 to 2, and most preferably 0.6 to 1.

7.

11. A composition comprising carbon black and expanded graphite, wherein the weight percent ratio of carbon black to graphite relative to the total weight of the composition is in the range of from 0.1 to 9, preferably from 0.33 to 9, more preferably from 0.4 to 9, even more preferably from 0.4 to 7, still more preferably from 0.4 to 5, especially more preferably from 0.4 to 3, especially even more preferably from 0.4 to 2, and most preferably from 0.6 to 1.7; Carbon black is 950m 2 ・g -1 Less than 850m, preferably 2 ・g -1 Less than 700m, more preferably 2 ・g -1 less than, and even more preferably, 600 m 2 ・g -1 Less than 500m, most preferably 2 ・g -1 less than, in particular 40 to 800, preferably 50 to 800, more preferably 30 to 100, even more preferably 50 to 80, most preferably 60 to 70 m 2 ・g -1 BET specific surface area under nitrogen measured according to ASTM D-3037 in the range of and, optionally, a primary particle size, measured according to ASTM D-3849-14a, of 10 to 60, preferably 15 to 55, more preferably 20 to 40, even more preferably 25 to 35 nm; and / or - 400ml / g -1 Less than 390 ml g -1 less than, more preferably 380 ml g -1 less than, and even more preferably less than 370 ml g -1 less than, most preferably 350 ml g -1 less than, in particular 100 to 330, preferably 150 to 230, more preferably 170 to 210, even more preferably 180 to 200, most preferably 185 to 195 ml g -1 and characterized by one or more oil absorption numbers OAN, as measured in accordance with ASTM D-2414, in the range of and / or Expanded graphite is a particle size distribution D, as measured according to ISO 13220, of from 5 to 1000, preferably from 20 to 800, more preferably from 30 to 700, even more preferably from 50 to 600, still more preferably from 70 to 500, particularly more preferably from 80 to 250, most preferably from 85 to 150 μm 90 and / or 0.01 to 1.00, preferably 0.02 to 0.9, more preferably 0.05 to 0.7, even more preferably 0.1 to 0.55, still more preferably 0.13 to 0.50, especially more preferably 0.16 to 0.45, most preferably 0.16 to 0.25 g cm -3 and a bulk density, as measured in accordance with ASTM D-7481, of

12. 12. The composition of claim 11, comprising carbon black in an amount of 3 to 40, preferably 5 to 35, more preferably 10 to 30, even more preferably 12 to 26, and most preferably 13 to 18% by weight, relative to the total weight of the composition.

13. 12. The composition according to claim 11, comprising expanded graphite in an amount of 3 to 50, preferably 3 to 40, more preferably 3 to 35, even more preferably 3 to 30, still more preferably 3.5 to 20, particularly more preferably 4 to 18, especially still more preferably 5 to 17, and most preferably 7 to 15% by weight, relative to the total weight of the composition.

14. 12. The composition of claim 11, comprising carbon black and expandable graphite in a combined amount of 10 to 50, preferably 17 to 45, more preferably 19 to 40, even more preferably 20 to 35, still more preferably 22 to 34, and most preferably 25 to 30 wt.%, based on the total weight of the composition.

15. 12. The composition of claim 11, comprising one or more fillers selected from the group consisting of carbon-based fillers selected from the group consisting of metal powders, metal flakes, glass fibers, silicon fibers, carbon conductive additives, natural graphite, artificial graphite, surface-modified graphite, graphite nanoplatelets, multi-walled carbon nanotubes, single-walled carbon nanotubes, carbon nanostructures, metal-coated graphite, and combinations thereof.

16. 12. The composition of claim 11, comprising a polymer, preferably a polyolefin, preferably a polymer selected from the group consisting of a polyolefin selected from polyethylene, propylene, and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethyl methacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymer, polyester, polycarbonate, polyketone, polysulfone, unsaturated polyester, polyurethane, polycyclopentadiene, silicone, rubber, thermoset resin, thermoplastic resin, coating binder, and combinations thereof.

17. 12. A composite molded article comprising the composition of claim 1 or 11, or a substrate coated with a coating comprising said composition.

18. 18. The shaped article or substrate coating of claim 17, comprising a polymer selected from the group consisting of polyolefins, preferably selected from polyethylene, propylene, and combinations thereof, more preferably the polyolefin is polypropylene, polyamide, polymethyl methacrylate (PMMA), polyacetal, polycarbonate, polyvinyl, polyacrylonitrile, polybutadiene, polystyrene, polyacrylate, epoxy polymer, polyester, polycarbonate, polyketone, polysulfone, unsaturated polyester, polyurethane, polycyclopentadiene, silicone, rubber, thermoset resin, thermoplastic resin, coating binder, and combinations thereof.

19. 20. The shaped article or coated substrate of claim 18, wherein the carbon black and expandable graphite are dispersed in the polymer.

20. an electromagnetic interference (EMI) shielding of at least 20 dB, preferably at least 30 dB, more preferably at least 40 dB, measured according to ASTM D-4935 at frequencies between 10 and 1000 MHz, or a method derived therefrom as detailed in the paper by E. Hariya and U. Massahiro, "Instruments for Measuring Shielding Effectiveness", EMC 1984 Tokyo; a volume resistivity, measured according to ASTM D-4496, of less than 1000 ohm-cm, preferably less than 100 ohm-cm, more preferably less than 10 ohm-cm, and most preferably less than 1 ohm-cm; and / or - 0.5 W m -1 K -1 More than 0.7 W m -1 K -1 More preferably, 0.9 W m -1 K -1 More preferably, it is greater than 1.1 W m -1 K -1 more preferably 1.3 W m -1 K -1 More preferably still, 1.5 W m -1 K -1 More particularly, more preferably 1.7 W m -1 K -1 More preferably, it exceeds 2.0 W m -1 K -1 More preferably, 2.5 W m -1 K -1 more preferably greater than 3.0 W m -1 K -1 more than 4.0 W m -1 K -1 more than 5.0 W m -1 K -1 More preferably, it exceeds 6.0 W m -1 K -1 More than 7.0 W m -1 K -1 12. Use of the composition of claim 1 or 11 to provide one or more in-plane thermal conductivities, measured in accordance with ASTM E1461, of greater than 1000 kJ / cm.sup.

2.

21. 12. A method for providing electromagnetic interference (EMI) shielding, measured in accordance with ASTM D-4935 at frequencies from 10 MHz to 1000 MHz, of at least 20 dB, preferably at least 30 dB, more preferably at least 40 dB, in a polymeric composition using the composition of claim 1 or 11.

22. 12. A method for providing a polymeric composition using a composition according to claim 1 or 11, wherein the polymeric composition has a volume resistivity, as measured according to standard test method ASTM D-4496, of less than 1000 ohm-cm, preferably less than 100 ohm-cm, more preferably less than 10 ohm-cm, and most preferably less than 1 ohm-cm.

23. In a polymeric composition using the composition of claim 1 or 11, the -1 K -1 More than 0.7 W m -1 K -1 More preferably, 0.9 W m -1 K -1 More preferably, it is greater than 1.1 W m -1 K -1 more preferably 1.3 W m -1 K -1 More preferably still, 1.5 W m -1 K -1 More particularly, more preferably 1.7 W m -1 K -1 More preferably, it exceeds 2.0 W m -1 K -1 More preferably, 2.5 W m -1 K -1 more preferably greater than 3.0 W m -1 K -1 more than 4.0 W m -1 K -1 more than 5.0 W m -1 K -1 More preferably, it exceeds 6.0 W m -1 K -1 More than 7.0 W m -1 K -1 1. A method for providing an in-plane thermal conductivity, measured in accordance with ASTM E1461, of greater than 1.

24. 22. A method of providing electromagnetic interference (EMI) shielding according to claim 21, wherein the EMI shielding is improved by at least 10 dB, preferably at least 20 dB, more preferably at least 25 dB, even more preferably at least 30 dB, still more preferably at least 35 dB, particularly more preferably at least 40 dB, and most preferably at least 45 dB, especially from 10 to 80 dB, preferably from 15 to 70 dB, more preferably from 18 to 60 dB, particularly more preferably from 20 to 55 dB, even more preferably from 25 to 50 dB, particularly even more preferably from 27 to 50 dB, even more preferably from 30 to 50 dB, particularly even more preferably from 31 to 45 dB, and most preferably from 35 to 42 dB, when compared to a reference material not containing carbon black, expanded graphite, or other conductive fillers or additives.

25. 1.3 to 10 when compared to a reference material containing no carbon black, expanded graphite, or other conductive fillers or additives 9 , preferably 1.5 to 10 8 , more preferably 2 to 10 7 , particularly preferably 2 to 10 6 , and even more preferably 2 to 10 5 , particularly still more preferably 3 to 10 5 , and even more preferably 3 to 10 4 , particularly still more preferably 5 to 10 4 , and even more preferably 7 to 10 4 , and even more preferably 7 to 10 3 , particularly even more preferably 10 to 10 3 , particularly still more preferably 15 to 10 3 , and even more preferably 50 to 10 3 , most preferably 10 2 ~10 3 23. The method of claim 22, wherein the volume resistivity is reduced by a factor of

26. 24. A method of providing thermal conductivity according to claim 23, wherein the thermal conductivity is increased by a factor of 2, preferably 3, more preferably 4, particularly preferably 5, even more preferably 6, particularly even more preferably 7, even more preferably 8, particularly even more preferably 9, even more preferably 10, even more preferably 12, particularly even more preferably 14, particularly even more preferably 16, even more preferably 18, even more preferably 20, particularly even more preferably 25, particularly even more preferably 30, even more preferably 40, and most preferably 50 when compared to a reference material not containing carbon black, expanded graphite or other conductive fillers or additives.

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